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In-Situ Synchrotron Radiation Study of Formation and Growth of Crystalline CexZr1-xO2 Nanoparticles Synthesized in Supercritical Water

Tyrsted, Christoffer ; Becker, Jacob ; Hald, Peter ; Bremholm, Martin ; Pedersen, Jan Skov ; Chevallier, Jacques ; Cerenius, Yngve LU ; Iversen, Steen B. and Iversen, Bo B. (2010) In Chemistry of Materials 22(5). p.1814-1820
Abstract
In situ synchrotron powder X-ray diffraction (PXRD) measurements have been conducted to follow the nucleation and growth of crystalline CexZr1-xO2 nanoparticles synthesized in supercritical water with a full substitution variation (x = 0, 0.2, 0.5, 0.8, and 1.0). Direction-dependent growth curves are determined and described using reaction kinetic models. A disctinct change in growth kinetics is observed with increasing cerium content. For x = 0.8 and 1.0 (high cerium content), the growth in initially limited by the surface reaction kinetics, however, at a size of similar to 6 nm, the growth changes and becomes limited by the diffusion of monomers toward the surface. For x = 0 and 0.2, the opposite behavior is observed with the growth... (More)
In situ synchrotron powder X-ray diffraction (PXRD) measurements have been conducted to follow the nucleation and growth of crystalline CexZr1-xO2 nanoparticles synthesized in supercritical water with a full substitution variation (x = 0, 0.2, 0.5, 0.8, and 1.0). Direction-dependent growth curves are determined and described using reaction kinetic models. A disctinct change in growth kinetics is observed with increasing cerium content. For x = 0.8 and 1.0 (high cerium content), the growth in initially limited by the surface reaction kinetics, however, at a size of similar to 6 nm, the growth changes and becomes limited by the diffusion of monomers toward the surface. For x = 0 and 0.2, the opposite behavior is observed with the growth initially being limited by diffusion (up to similar to 3.5 nm) and later by the surface reaction kinetics. Thus, although a continuous solid solution can be obtained for the ceria-zirconia system, the growth of ceria and zirconia nanoparticles is fundamentally different under supercritical flow reactor. The resulting samples were analyzed using PXRD, small-angle X-ray scattering (SAXS), and transmission electron microscopy (TEM). The nanoparticles with x = 0, 0.2, and 0.5 have very low polydispersities. The sizes range from 4 nm to 7 nm, and the particles exhibit a reversibly pH-dependent agglomeration. (Less)
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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Chemistry of Materials
volume
22
issue
5
pages
1814 - 1820
publisher
The American Chemical Society (ACS)
external identifiers
  • wos:000274929000028
  • scopus:77949343598
ISSN
0897-4756
DOI
10.1021/cm903316s
language
English
LU publication?
yes
id
a5446d58-a901-49bb-a616-e50bac1a0e42 (old id 1568287)
date added to LUP
2016-04-01 10:19:02
date last changed
2022-04-04 08:49:58
@article{a5446d58-a901-49bb-a616-e50bac1a0e42,
  abstract     = {{In situ synchrotron powder X-ray diffraction (PXRD) measurements have been conducted to follow the nucleation and growth of crystalline CexZr1-xO2 nanoparticles synthesized in supercritical water with a full substitution variation (x = 0, 0.2, 0.5, 0.8, and 1.0). Direction-dependent growth curves are determined and described using reaction kinetic models. A disctinct change in growth kinetics is observed with increasing cerium content. For x = 0.8 and 1.0 (high cerium content), the growth in initially limited by the surface reaction kinetics, however, at a size of similar to 6 nm, the growth changes and becomes limited by the diffusion of monomers toward the surface. For x = 0 and 0.2, the opposite behavior is observed with the growth initially being limited by diffusion (up to similar to 3.5 nm) and later by the surface reaction kinetics. Thus, although a continuous solid solution can be obtained for the ceria-zirconia system, the growth of ceria and zirconia nanoparticles is fundamentally different under supercritical flow reactor. The resulting samples were analyzed using PXRD, small-angle X-ray scattering (SAXS), and transmission electron microscopy (TEM). The nanoparticles with x = 0, 0.2, and 0.5 have very low polydispersities. The sizes range from 4 nm to 7 nm, and the particles exhibit a reversibly pH-dependent agglomeration.}},
  author       = {{Tyrsted, Christoffer and Becker, Jacob and Hald, Peter and Bremholm, Martin and Pedersen, Jan Skov and Chevallier, Jacques and Cerenius, Yngve and Iversen, Steen B. and Iversen, Bo B.}},
  issn         = {{0897-4756}},
  language     = {{eng}},
  number       = {{5}},
  pages        = {{1814--1820}},
  publisher    = {{The American Chemical Society (ACS)}},
  series       = {{Chemistry of Materials}},
  title        = {{In-Situ Synchrotron Radiation Study of Formation and Growth of Crystalline CexZr1-xO2 Nanoparticles Synthesized in Supercritical Water}},
  url          = {{http://dx.doi.org/10.1021/cm903316s}},
  doi          = {{10.1021/cm903316s}},
  volume       = {{22}},
  year         = {{2010}},
}